Previous investigations have identified the correlation between synthetic conditions and soft nanoparticle morphology, including their molecular weight, internal crosslinked structure, total nanoparticle radius, and topology, or degree of “fuzziness” of each nanoparticle. To provide further insight to these guidelines, we examine the effect of surfactant concentration and monomer water solubility on the topology, size, and polydispersity of soft poly(butyl acrylate) nanoparticles. Small-angle neutron scattering studies confirm that increased monomer water solubility and polymer chain flexibility decreases the control of nanoparticle topology and size in a nano-emulsion polymerization. Further studies document the morphological change of polystyrene soft nanoparticles with a decrease in solvent quality. Small-angle neutron scattering was also used to characterize dilute solutions of soft polystyrene nanoparticles in a good and theta solvent, including the analysis of their internal structure. When the soft nanoparticles are dispersed in a thermodynamically good solvent they exhibit a swollen morphology, however, when dispersed in a theta solvent, the nanoparticle core contracts due to unfavorable thermodynamic interactions. Moreover, the structure of soft nanoparticles in a theta solvent provides insight that will guide the interpretation of the behavior of soft nanoparticles dispersed into a bulk polymer matrix.