An efficient simulator for quantum systems is one of the original goals for the efforts to develop a quantum computer [1]. In recent years, synthetic dimension in photonics [2] have emerged as a potentially powerful approach for simulation that is free from the constraint of geometric dimensionality. Here we demonstrate a quantum-correlated synthetic crystal, based upon a coherentlycontrolled broadband quantum frequency comb produced in a chip-scale dynamically modulated lithium niobate microresonator. The time-frequency entanglement inherent with the comb modes significantly extends the dimensionality of the synthetic space, creating a massive nearly 400 × 400 synthetic lattice with electrically-controlled tunability. With such a system, we are able to utilize the evolution of quantum correlations between entangled photons to perform a series of simulations, demonstrating quantum random walks, Bloch oscillations, and multi-level Rabi oscillations in the time and frequency correlation space. The device combines the simplicity of monolithic nanophotonic architecture, high dimensionality of a quantum-correlated synthetic space, and onchip coherent control, which opens up an avenue towards chip-scale implementation of large-scale analog quantum simulation and computation [1, 3, 4] in the time-frequency domain.