I won't argue "greatest", but right up there was
this one. Some of the most fun I've ever had watching what became a loss for my team*. And everyone said "what a thrill - can't wait till the rematch", and then we came within a game of making that happen.
* right up there Sean Manaea no-hitting our eventual-champion 2018 Sox.
Regular season only, that game against SF represented the most passing yards Brady had ever thrown in a loss. 443 pass yards on 65 (!) attempts.
And I know it's been mentioned here or in the Brady thread, but he threw 50+ passes 39 times in his career - counting both regular season and post season. Of those 39 times:
reg season: 29 times, 19 wins, 10 losses
post season: 10 times, 6 wins, 4 losses
So 39 times throwing 50+ passes: 25 wins, 14 losses, .641
That's absolutely insane.
EDIT: Just for comparison's sake, here's the same data for Peyton Manning.
reg season: 17 times, 4 wins, 13 losses
post season: 0 times
But he did throw 40+ times in the postseason 12 times and went 3-9 in those games.
For the vast majority of QBs, throwing a ton of passes happens in losing efforts. But for Brady, it usually led to victories. Overwhelmingly so actually. And a large data pool to observe. The opposite of being a "system quarterback", it turned out that more than anyone else, teams rode Brady's arm to victory.