Goals from Sergio Aguero and Kevin De Bruyne secured a 2-0 win for City over Sheffield United on Sunday, though it was not without controversy.
VAR harshly disallowed a would-be opener from Lys Mousset, while referee Chris Kavanagh seemed to inadvertently block John Fleck in the lead up to Aguero’s 52nd-minute strike.
The triumph brought up a century of Premier League wins for Guardiola in his 134th top-flight match in charge of City.
Current Spurs boss Mourinho had previously held the record, having achieved 100 wins in 142 games, while Liverpool manager Jurgen Klopp managed to do so in 159 matches earlier this month.
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