To adapt to the operational requirements of the wide temperature range environment-for the single-based propellant, this work investigated the modification effects of temperature coefficient of propellant through physical structure modification, insensitive technology, and surface modification methods. Here, the prepared propellant was evaluated by the internal ballistic performance test. The low temperature velocity temperature coefficient and high temperature chamber pressure temperature coefficient could be controlled below 5% and 10%, respectively when the propellant was modified with 5% pore extender, a particle size of energetic solid material of 55 μm, the insensitive agent MA, and surface sensibilization modification. The modification mechanism for the propellant towards these methods is attributed to that the pores, irregular bulge, open interface, and zipper hole section structure are formed. Hence, at the lower temperature-condition, because of the porous layer and PMA of the propellant becoming brittle, the impact resistance being weakened, the fracture tendency of the pores and the interface being increased, the initial burning surface of the propellant was increased at low temperature. At the lower temperature condition, because of the closed hole phenomenon of the propellant blocked (closed) hole layer being intensified, insensitive agent being expanded and squeezed into the hole, the impact resistance being enhanced, the fracture tendency of the pore and the interface being reduced, the initial burning surface of the propellant was reduced under high temperature conditions. Through the compensation of the burning rate, the aim of adjusting the temperature coefficient of the propellant is achieved.