United lost to second-tier Derby County in the League Cup on Tuesday before a humbling afternoon at the London Stadium.
A fifth-minute strike from Felipe Anderson and a Victor Lindelof own goal put West Ham 2-0 up before half-time.
Second-half substitute Marcus Rashford pulled a goal back for United before Marko Arnautovic sealed the win for the home side.
Mourinho's relationship with star midfielder Paul Pogba will once again be in the spotlight after the Frenchman was substituted in the 71st minute.
Earlier this week, Mourinho stripped the World Cup-winning midfielder of his vice captaincy role before footage emerged which appeared to show the two having a disagreement on the training ground.
The defeat means United sit eighth in the table, eight points behind early leader Liverpool which faces Chelsea later in the day.
After winning the Europa League, and League Cup in first season at United, Mourinho led the Red Devils to a second-place finish in the Premier League last season -- albeit 19 points behind fierce local rivals Manchester City.
Now in his third season at the club, Mourinho has been heavily criticized for poor results and for the team's conservative style of play.
This latest defeat means United has lost three of its opening seven Premier League games.
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