The rapid growth and development of manufacturing technology for controlling processors and high-power semiconductor devices has led to the enhancement of flexible AC transmission system (FACTS) controllers, thus improving the performance of power systems. The generalized unified power flow controller (GUPFC) is today introduced as the most advanced generation of the FACTS family, which is based on voltage source converter (VSC). It can, hence, control all the five parameters of a powersystem given above. The paper, for the first time, presents the accurate modeling of different parts of the control system and power electronics of the 72-pulse VSC-based GUPFC in detail to satisfy operation constraints and improve power quality in terms of harmonic level reduction. There is no need to use active or passive filters in the proposed model for reducing harmonic level of the GUPFC. In this regard, the calculation of four main parameters, namely D_alpha, alpha, angular speed, and sigma, as inputs of the pulse-firing system for the 72-pulse VSC is performed dynamically and optimally to meet all expected constraints in terms of operation, power quality, and harmonic reduction of a network with a GUPFC. The presented modeling is implemented on a 230 kV GUPFC-compensated double-circuit transmission line in MATLAB/Simulink environment, andthe desired results of the presence of the 72-pulse VSC-based GUPFC are shown to meet the desired constraints of operators