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A series of polycrystalline Ca(3)Co(2-x)Mn(x)O(6) with 0.93 < x < 1.07 are prepared in order to investigate the effect of Co:Mn ratio around x similar to 1.0 on the multiferroicity. It is found that the ferroelectric polarization P at low temperature shows significant dependence on the Co:Mn ratio, forming a V-shaped pattern with the lowest point at x similar to 0.99. It is proposed that the suppression of P with the Co:Mn ratio approaching to the best Co/Mn order originates from the disruption of the long range spin order. (C) 2010 American Institute of Physics. [doi: 10.1063/1.3464289]