The mechanical properties of network molecular systems, prepared through visible (Ar+) laser-induced polymerization of multifunctional acrylates, were studied as a function of some of the photopolymerization parameters. The properties investigated were the Young’s modulus of elasticity and the stress-at-break, both derived from the stress versus strain test of dogbone-shaped photopolymerized samples. The parameters studied included the dye and co-initiator concentrations, and the laser power. We also compared the mechanical properties of samples made using different types of fluorone dyes and using two different amines as co-initiator. Better polymers are formed by the dyes with low fluorescence quantum yield. The three photopolymerization parameters modify the mechanical properties in a very similar way : they initially tend to increase both the Young’s modulus and the stress-at-break but have a deleterious effect on the material strength if used in excess. N-phenylglycine, NPG, was shown to form stronger polymers (higher Young’s modulus) than if N,N-dimethyl-2,6-diisopropylaniline, DIDMA, was used as co-initiator. We discuss the possible molecular mechanisms for such observations.