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 coherently-controlled 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 x 400 synthetic lattice with electrically-controlled tunability. With such a system, ...