Nanoimprint lithography is a newly developed patterning method that employs a hard template for the patterning of structures at micro- and nanometer scales. This technique has many advantages such as cost reduction, high resolution, low line edge roughness (LER), and easy operation. However, resist peeling, defects, low degree of planarization, and low throughput issues present challenges that must be resolved in order to mass produce advanced nanometer-scale devices. In this study, the new approach of using a silicon-containing spin-on hard mask underlayer material with high adhesion by reacting methacrylate groups of the underlayer to the acrylate groups of resist material during ultraviolet irradiation was demonstrated to obtain the excellent patterning dimensional accuracy and increase the process latitudes. The performance of this process is evaluated by using step and flash imprint lithography. The obtained high adhesion between the underlayer and resist material was found to lead a silicon-containing underlayer material to excellent patterning dimensional accuracy and 80 nm straight profiles. We expect that the silicon-containing a spin-on hard mask material under organic resist will be one of the most promising materials in the next generation of nanoimprint lithography.