The 30-year-old, who won the 2020 award and was runner-up last year, polled 31 votes to win from the Western Bulldogs' Marcus Bontempelli (29) and Collingwood's Nick Daicos (28), storming home with three-vote games in the final two rounds.
Neale is the first two-time winner since former Fremantle teammate Nat Fyfe in 2015 and 2019, and just the 16th player to win multiple Brownlow Medals.
He is also the first player to win the top award without being named in the All-Australian team since former West Coast midfielder Matt Priddis in 2014.
The superstar Lion, who will play a key role against Collingwood in Saturday's decider, averaged 27.4 disposals, 8.1 clearances and 13.9 contested possessions across the regular season.
"Yeah it doesn't sit very well, at the moment," a shocked Neale said from the Lions' Brownlow function in Brisbane.
"I'm sure it will sink in at a later date. I'm pretty rattled to be honest. So apologies if this (interview) doesn't go too well.
"I did not expect this, and to be amongst some of those names that have won two is unbelievable."
Sydney's Errol Gulden and Port Adelaide star Zak Butters rounded out the top five with 27 votes apiece.
The final rounds were extraordinarily dramatic.
Dashing 20-year-old Daicos, son of Collingwood great Peter Daicos, was a red-hot favourite for most of the season but missed the final three rounds after suffering a hairline fracture in his knee during round 21.
Remarkably, the young gun led on 28 votes after round 18 and held that lead until round 23, despite not polling in that time.
Neale drew level with Daicos in round 23, with Bontempelli, Errol Gulden and Christian Petracca locked on 26 heading into the final round.
Bontempelli, who was also runner-up to Ollie Wines in 2021, claimed three votes in his final game, but was leapfrogged by Neale's best-on-ground performance against St Kilda.
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