The title-chasing Gunners led the Hammers 1-0 in injury time, until Callum Wilson struck a last-gasp leveller. However, the goal - which would have boosted West Ham's survival hopes and dented Arsenal's title chances - was subsequently ruled out for a foul on goalkeeper David Raya.
Speaking on Sky Sports' commentary during the game, Neville said: "This is an earthquake, a tremor of a moment.
"Arsenal Football Club's first title in 22 years could rest on this. This is one of those moments where Arsenal might think their name is on the trophy...
"VAR Darren England is the FA Cup referee. He won't face a more pressurised moment than that at Wembley."
Arsenal ultimately held on for the win, meaning they can secure the championship with victories in their final two fixtures of the league campaign.
Despite this, the VAR call dominated the post-match chat, with the decision dividing fans and pundits.
Roy Keane, the former Manchester United captain, said on Sky Sports: "The one thing you say when you go up, VAR are going to check everything, do not put your hands on the goalkeeper! Certainly don't leave it on for three or four seconds.
"There is all sorts going on but because the goalkeeper had such a big part to play, I think it is a foul. It was really silly from West Ham. Don't make it such an obvious foul because they are going to check."
Neville also reflected on referee Dan England after the game.
The former England international said on The Gary Neville Podcast: "I think that's the biggest moment in VAR history in the Premier League.
"There are a lot who aren't fans of VAR, and maybe rightly so, but it could have just made Arsenal champions, and it could have got a decision right that wouldn't have been right.
"I was wondering whether Darren England had the courage, had the nerve to overturn, and what was he going to do in this moment. I have to say we get the luxury, and I wish all fans at home and fans in the stadium got the luxury of being able to hear them, because to be fair he was composed, he was walking through it, he was talking to the referee, he was talking to his colleague who was sat next to him, and he walked through it perfectly."
