We use trapped atomic ions forming a hybrid Coulomb crystal, and exploit its phonons to study an isolated quantum system composed of a single spin coupled to an engineered bosonic environment. We increase the complexity of the system by adding ions and controlling coherent couplings and, thereby, we observe the emergence of thermalization: Time averages of spin observables approach microcanonical averages while related fluctuations decay. Our platform features precise control of system size, coupling strength, and isolation from the external world to explore the dynamics of equilibration and thermalization.