Following a 1-1 draw in the first leg, the Spaniards travelled to the Emirates Stadium hoping to secure a positive result and book their place in the final.
However, it was Mikel Arteta’s men who progressed, thanks to a decisive first-half strike from Bukayo Saka.
Despite the disappointment, the Argentine coach said he was proud of his team’s effort, saying they gave everything.
"If we got knocked out, it's because our opponents deserved to get through,” Simeone said after the game, per Amazon Prime.
“They took their chances, including their big chance in the first half, and they deserved to get through. If you ask me how I feel, I feel calm and peaceful. The team gave absolutely everything."