We report the development of an efficient many-body algorithm for simulating open quantum system dynamics that utilizes a time-dependent variational principle for matrix product states to evolve large system-environment states. Capturing all system-environment correlations, we reproduce the nonperturbative, quantum-critical dynamics of the zero-temperature spin-boson model, and then exploit the many-body information to visualize the complete time-frequency spectrum of the environmental excitations. Our “environmental spectra” reveal correlated vibrational motion in polaronic modes which preserve their vibrational coherence during incoherent spin relaxation, demonstrating how environment information could yield valuable insights into complex quantum dissipative processes.