We report here on the multiferroic properties of ZnO–BiFeO3 (BiFeO3 referred hereinafter as BFO) nanocomposite structures obtained by using a facile solution-based synthesis route. ZnO is found to grow in the form of well-crystallized and self-assembled dumbbell-like structures. BFO nanoparticles (NPs) are deposited onto ZnO nanodumbbells (NDs) to obtain ZnO–BFO heterostructures. The nanocomposites show prominent ferroelectric polarization hysteresis loop along with enhanced magnetization in comparison to pure BFO NPs. The ordered alignment of spins along with the suppression of Fe–O–Fe antiferromagnetic super-exchange interactions at the ZnO/BFO interface plausibly gives rise to observed multiferroic properties.