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Abstract Adaptive Variational Quantum Dynamics (AVQD) algorithms offer a promising approach to providing quantum‐enabled solutions for systems treated within the purview of open quantum dynamical evolution. In this study, the unrestricted‐vectorization variant of AVQD is employed to simulate and benchmark various non‐unitarily evolving systems. Exemplification of how construction of an expressible ansatz unitary and the associated operator pool can be implemented to analyze examples such as the Fenna–Matthews–Olson complex (FMO) and even the permutational invariant Dicke model of quantum optics. Furthermore, an efficient decomposition scheme is shown for the ansatz used, which can extend its applications to a wide range of other open quantum system scenarios in near future. In all cases the results obtained are in excellent agreement with exact numerical computations that bolsters the effectiveness of this technique. The successful demonstrations pave the way for utilizing this adaptive variational technique to study complex systems in chemistry and physics, like light‐harvesting devices, thermal, and opto‐mechanical switches, to name a few.