Using a high temperature vaporizing spray approach to nanoparticle fabrication, we reveal a straightforward process for the formation of polyethyleneimine (PEI) scaffold based hydrogel nanoparticles. With PEI as the polymeric skeleton, we demonstrate the possibility for capture and release of small molecule, protein, nucleic acid, or colloidal cargo. Here, we provide evidence for use of the PEI nanoparticles as versatile nanocarriers. Moreover, we provide characterization of the nanoparticles produced by our inductive heat spraying approach along with determination of the loading capacity for the various cargos. We also observed the release profiles for a traceable small molecule in our proof of concept work. While linear chains or dendrimers of PEI are well-known to be cytotoxic, we revealed that our larger scale nanoparticles (which are in the range of 400-500 nm) have no noticeable cytotoxicity in vitro. With this initial work, we expect the intrinsic capabilities of the PEI nanoparticle scaffold demonstrated here in terms of molecular capture may possibly be utilized for effective nanocarriers upon future tuning of the nanoparticle size as to avoid any rapid clearance.