With Kohei Horikoshi's My Hero Academia having an extensive cast, several characters with unique traits and personalities have emerged throughout the entire series. While the heroes of the series have always been the focal point of drawing attention, the villains have created a fan base of their own.
With the series already giving redemption to some of the popular villain characters, like Gentle Criminal, La Brava, and Lady Nagant, several other villains have somehow shown that they also deserve redemption. Some villains stayed true to their nature and exhibited no redeemable qualities. Here's a list of villains who could be redeemed, and some who are lost causes.
Disclaimer: This article solely reflects the author's opinions.
Toga, Kurogiri, and 3 other My Hero Academia villains who could be redeemed
1) Himiko Toga

During her final moments in the series, Himiko Toga felt a strong wave of emotional change after Ochaco Uraraka reached out to her. Despite her villainous acts throughout the series, Uraraka told Toga that she finally understood Toga's true feelings and affections. This made Toda sacrifice herself by transferring all her blood to an injured Ochaco, as an act of selflessness and love for her.
Her final actions defined Toga more like the person she was, rather than just another villain in the series. In the end, her acts were not inherently villainous, but were the effects of the distorted pain she received throughout her life. If she were to have survived after giving away her blood, she definitely could have been redeemed.
2) Shigaraki Tomura

Despite being one of the main villains of the series, Shigaraki Tomura wasn't acting out of an evil nature, as commonly seen for several other villains in the My Hero Academia series. Tenko Shimura, Shigaraki's childhood name, was a child who was suffering from the trauma of accidentally killing his parents and was abandoned by society, which was exploited by All for One, filling him with hate.
Shigaraki's villainous descent cannot be completely held as his responsibility. If any hero had reached out to him, or even if anyone had shown him the support he needed, he could have walked on a different path. After Midoriya destroyed All for One's vestige, Tomura found peace and was no longer consumed by hatred. He was finally free from all the hate and destruction imposed by All for One.
3) Kurogiri

Kurogiri is a creation of All for One and Kyudai Garaki using the corpse of Oboro Shirakumo. Oboro was a classmate and friend of Shota Aizawa (Erasure Head) and Hizashi Yamada (Present Mic). During his Hero-Work studies, Oboro was killed by the villain Garvey, who was later revealed as an event orchestrated by All for One to gain Shota's Erasure Quirk.
During the final battle, after his Oboro personality started to resurface, despite being a major villain of the series, Kurogiri used his Warp Gate quirk to teleport the heroes to Mt. Fuji to assist Midoriya in the battle. Kurogiri's actions in the end showed how he could be redeemed, as his actions significantly changed the course of the battle against All for One and Tomura Shigaraki.
4) Spinner

Another villain whose descent was not entirely his fault, but partially can be blamed on society. Spinner, being a mutant, was treated with discrimination alongside other mutants in the series, forced to live as outcasts away from the cities. Spinner's accumulated hatred from the mutant discrimination led him to lead the raid on the hospital during the Final War arc.
After the final war, Spinner came in contact with Izuku Midoriya. While he still bore hatred toward Midoriya for killing Tomura, after hearing Shigaraki's final words, Spinner broke down emotionally. While he might not have been forgiven by many for what he did, a certain sense of empathy radiates from his reasoning to become a villain, deserving of a second chance.
5) Twice

In his early years, Jin Bubaigawara, also known as Twice, lost his parents to a villain's attack, becoming an orphan when he was in middle school. Later, he was convicted of wrongful accusations, which led to him losing his job and forced him into homelessness. While he was one of the major antagonists of the series, he showed signs of empathy and emotions throughout the series.
After his death at the hands of Hawks, the fandom went into debate over whether his death was necessary or not, turning it into a controversy. While he was still a villain near the end, Twice's character showed several personality changes that could have led to him redeeming himself. He could easily have been convinced to join the good side because of his character as a human being.
Overhaul, Muscular, and 3 other My Hero Academia villains who were lost causes
1) Overhaul

One of the most irredeemable villains of the series, Overhaul, played the role of a true villain, committing several heinous crimes throughout his time in the series. Torturing Eri to obtain her quirk, mass murder, manipulation of the mentally unstable individuals, killing Magne, and manufacturing the quirk-destroying bullet; the list goes on for crimes committed by Overhaul.
Even during his final moments, Overhaul did not show any remorse or repentance for his actions before being defeated by Deku. Kai showed no redeemable qualities and stayed true to his evil villain nature till the very end.
2) All for One

Being the main overarching antagonist and villain of the series, All for One's character is the ultimate embodiment of villains in the entire series. One of the most wicked and powerful characters from the series, All for One, does not possess even the slightest emotional capabilities of showing regret and remorse. Rather, he was very proud of his evil accomplishments.
From manipulation to straight-up killing several individuals while causing mass destruction, no redeemable qualities could be found for All for One. Even in his final moments before ceasing to exist, All for One showed extreme rage and grasped onto every possibility to destroy the heroes.
3) Muscular

Being the primary antagonist of the Forest Training Camp arc, Goto Imasuji, also known as the villain Muscular, is one of the more heinous criminals of the series. From killing the superhero team Water Hose to attacking cities, his list of crimes goes on. While he nearly killed Shindo, he expressed how much he loved killing and causing destruction.
Muscular showed no redeemable qualities as he was stern in his act of being the evil villain who causes mass destruction and loves to kill. While he was defeated by Midoriya during his attack on the training camp, he still clung to his evil persona and displayed no regret or remorse for his actions.
4) Re-Destro

Re-Destro is one of the My Hero Academia villains who shows no remorse or regret for his actions and holds no true moral compass. From justifying mass violence as righteous to having a frantic devotion to a flawed ideal, Re-Destro shows no qualities or behavioral traits to grant him redemption.
While maintaining a public moral facade as the CEO of the Detnerat Company, Re-Destro secretly was the grand commander of the Meta Liberation Army. When the merger happened with Tomura's League of Villains, Re-Destro became one of the nine lieutenants of the Paranormal Liberation Army, causing massive destruction and deaths of several heroes.
5) Kyudai Garaki- Doctor

While not leading the attacks from the frontlines, Kyudai Garaki, also known as Doctor, committed several villains acts while breaking several moral codes and laws from the shadows. He was the right-hand man of All for One, who was responsible for the creation of the Nomus and also created Kurogiri from Oboro's corpse.
He was also responsible for the modification of Tomura Shikaraki and integrating All for One inside of Shigaraki. He showed no remorse for his actions in using the corpses to create the Nomus, or even for killing people in the name of science. He was a psychopath who showed no redeemable qualities due to his lack of understanding of moral values in the first place.
Final thoughts
The My Hero Academia universe is filled with villains who, despite their crimes, have shown regret and tried to redeem themselves by trying to act to help others, rather than hurting them. While several villains had a change of heart when they got the opportunity, some were just evil and too far gone.
With the conclusion of the Final War arc yet to be revealed in the anime, several villains are yet to be featured, showing acts that might determine whether they can be redeemed.
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