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In the present work, the magnetic properties of a single crystal (Fe1–xMnx)2Mo3O8(0 ≤ x≤ 1) have been studied by performing extensive measurements. A detailed magnetic phase diagram is built up, in which the antiferromagnetic state dominates for x≤ 0.25 and the ferrimagnetic phase arises for x≥ 0.3. Meanwhile, a sizeable electric polarization of spin origin is commonly observed in all samples, no matter what the magnetic state is. For the samples hosting a ferrimagnetic state, square-like magnetic hysteresis loops are revealed, while the remnant magnetization and coercive field can be tuned drastically by simply varying the Mn content or temperature. A possible coexistence of the antiferromagnetic and ferrimagnetic phases is proposed to be responsible for the remarkable modulation of magnetic properties in the samples.