The bioaccumulation potential of contaminants in marine environments was investigated in biofilms and compared with caged mussels for a wide range of both organic and metallic contaminants across a large geographic area. Marine biofilms were sampled after three months of sub-surface immersion at 49 locations along the 1,800 km of the French Mediterranean coast. Ten chemical elements (i.e. As, Cd, Co, Cr, Cu, Hg, Mn, Ni, Pb, and Zn) and 57 organic compounds (i.e., 18 polycyclic aromatic hydrocarbons (PAHs), 8 dioxin-like and 6 non-dioxin-like polychlorinated biphenyls (PCBs) and 25 organochlorine pesticides (OCPs)) were quantified in triplicates, revealing different multi-contaminated profiles depending on sites. Most of contaminants exhibited higher concentrations in biofilms than in mussels. Moreover, a remarkable significant and positive correlation between the concentrations in both biological matrices was observed for PAHs and PCBs, and more contaminant-dependent for OCPs and metals. These results highlighted the potential of biofilms as relevant bioindicators of the marine chemical contamination.