Polymer-ceramic nanocomposites have been thoroughly investigated previously for high energy storage devices. However, the increase in performance of these nanocomposites has proven to be significantly lower than predicted values. Through surface functionalization of high dielectric constant nanoparticles (NP), the flaws that reduce composite performance can be eliminated to form high energy density composite materials. Functionalization methods utilize high throughput printing and curing techniques (i.e., inkjet printing and xenon flash lamp curing) that are crucial for rapid adoption into industrial production. (Ba,Ca) (Zr,Ti)O3 NPs (50 nm) are synthesized through the solvothermal method and functionalized with alkene terminated methoxysilanes. A thiol-ene monomer ink system, PTD3 [pentaerythritol tetrakis (3-mercaptopropionate) (PEMP, P), 1,3-Diisopropenylbenzene (DPB, D), 2,4,6-Triallyloxy-1,3,5-triazine (TOTZ, T)], is used as a high breakdown polymer matrix. Neat polymer, alkene terminated NP-polymer composites, and hydrophilic, TBAOH functionalized NP-polymer composites were spin coated onto both copper laminated glass slides and printed onto copper substrates in 1 cm(2) patterns for testing. Alkene functionalized NPs increased the breakdown strength by ∼38% compared to the nonfunctionalized NPs. Functionalized NPs increased both the breakdown strength and dielectric constant compared to the neat polymer, increasing the energy density nearly 3-fold from 13.3 to 36.1 J·cm(-3).