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Milan had 11 shots to Napoli's three in a dominant first half, but the visitors went ahead shortly after the break when Matteo Politano stroked home from 12 yards following Sergino Dest's clumsy foul on Khvicha Kvaratskhelia.
⚽️GOAL!! @_OlivierGiroud_ to the rescue as @acmilan gets the equaliser!
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Olivier Giroud pulled Milan level in the 69th minute, but substitute Simeone popped with the winner to seal a huge victory for Luciano Spalletti's side, who remain unbeaten in the league this season.
⚽️GOAL!! A predator's finish from new signing Giovanni Simeone and @en_sscnapoli is back in front against @acmilan!
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The result means Napoli leapfrogged Udinese and Atalanta at the top of the table, while Milan dropped down to fifth after a first Serie A defeat in 23 games.
Milan started strongly and were denied a 13th-minute lead when Giroud's strike from 12 yards was superbly tipped onto the crossbar by Alex Meret.
The Napoli goalkeeper was called into action again shortly before the half-hour mark when he pushed over Rade Krunic's header from a corner.
Napoli offered almost no attacking threat in the first half, yet they went ahead 10 minutes after the interval when Politano scored from the spot after substitute Dest had fouled Kvaratskhelia – the decision given after referee Maurizio Mariani was told to check the pitch-side monitor by VAR.
Meret denied Junior Messias soon after, before Giroud pulled Milan level with a simple finish from eight yards after fine work down the left by Theo Hernandez.
Its joy was short-lived, however, as Simeone stole into the area to glance home Mario Rui's cross from the left wing.
Milan should have snatched a point with four minutes remaining, yet substitute Pierre Kalulu inexplicably crashed against the crossbar with only Meret to beat from eight yards.