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The complex title salt, (C21H20OP)2[CoCl4], is the reaction product of CoCl2 with acetonyltriphenylphosphonium chloride in acetonitrile. In the anion, the CoII atom exhibits a typical tetrahedral environment, with Co—Cl distances ranging from 2.2721 (6) to 2.2901 (6) Å, and with Cl—Co—Cl angles ranging from 106.12 (2) to 112.24 (2)°. The two phosphonium cations likewise show the expected tetrahedral configuration, with P—C distances ranging from 1.785 (2) to 1.8059 (18) Å and C—P—C angles ranging from 106.98 (8) to 112.85 (15)°. The molecules interact in the lattice mainly through Coulombic and van der Waals forces because there is no particular polarity to the charges carried by the cations or anion. In the crystal, the cations and anions are arranged in sheets parallel to (001).