The crystal structures and electronic transport properties of composites, xLa5/8Ca3/8MnO3 (1-x)ErMnO3 (x=0, 0.2, 0.4, 0.5, 0.6, 0.8, 1), where ErMnO3 is the insulating ferroelectric and La5/8Ca3/8MnO3 is the metallic ferromagnetic component, were studied. The magnetization of samples (x=0, 0.5, 1) were also measured as a function of temperature from 4 K to 300 K. The X-ray diffraction data show La5/8Ca3/8MnO3 and ErMnO3 are almost complete immiscible, originating from the significant difference in their crystal structures. All the composites show a metal-insulator transition when the molar fraction of xLa5/8Ca3/8MnO3 component x≥0.4 and the electronic transport behaviors follow the classical percolation theory model very well. Magnetization of the mixture with x=0.5 is unique and enhanced greatly compared with that of pure ErMnO3. Comprehensive analysis of the electronic transport and magnetic results suggests that this material system is a new kind of multiferroic with stronger magnetism in a wider temperature range compared with the single phase multiferroic ErMnO3.