The manager had become dismayed by the club's transfer strategy this summer, leaving Keith Millen to take charge of the first team for Saturday's match against Arsenal.
The 56-year-old had become disillusioned with Palace’s transfer strategy this summer and held showdown talks with the club’s co-chairman Steve Parish on Thursday.
Keith Millen will take charge of the first team for Palace’s Premier League opener against Arsenal at the Emirates Stadium on Saturday.
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Palace has completed deals for four players this summer but only Fraizer Campbell and Martin Kelly were cash purchases, with Chris Kettings and Brede Hangeland arriving as free transfers.
Pulis had clashed with Parish on numerous occasions this summer over the club’s transfer policy, having missed out on deals for Gylfi Sigurdsson and Steven Caulker.
Pulis, who was named as the Premier League’s manager of the year in May, took over from Ian Holloway in November with Palace in the bottom three but was able to guide the club to an 11th-place finish.