After Federico Dimarco had given the hosts an early advantage, a brilliant first-time strike from Paulo Dybala ensured the scores were all level at half-time.
An eventful second half could have sen the game go either way, but ultimately it was Smalling who delivered the decisive moment; heading home from Lorenzo Pellegrini's inswinging free-kick to clinch an invaluable three points.
That was not Smalling's only late intervention; the centre-back finding himself in the right place at the right time to clear away substitute Robin Gosen's goalbound header.
Inter thought they had found the lead inside the first 10 minutes, only for Edin Dzeko's low finish to be ruled out by VAR following an offside in the build-up.
Dimarco nevertheless gave the Nerazzurri the lead soon after, only for Dybala to finish expertly from a well-weighted cross from Leonardo Spinazzola to restore parity in the contest.
Inter had their chances in the second half - Calhanoglu hitting the crossbar from a free-kick, with Lautaro also often dangerous - but Roma stayed in the contest, and got their reward when Smalling emphatically finished off from close range.
The Giallorossi are back in action on Thursday night, with Real Betis visiting the Stadio Olimpico in the UEFA Europa League.
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