Heralded single-photon source (HSPS) intrinsically suffers from the trade-off between the heralded single-photon rate and the single-photon purity. To break through this trade-off, one can apply multiplexing technology in different degrees of freedom that significantly improves the performance of the HSPS. Here, we propose a 1.5 μm chip-scale HSPS on lithium niobate on insulator by employing spectral multiplexing and active feed-forward spectral manipulating, and we demonstrate a proof-of-principle experiment with discrete fiber-based components. With continuous-wave laser pumping and three spectral modes multiplexed, our experimental results show that the spectral multiplexing improves the heralded single-photon rate by near threefold while keeping the g(2)(0) as low as 0.0006±0.0001 at a measured single-photon rate of 3.1 kHz. By measuring the joint spectral intensity, we show that the spectral multiplexing and feed-forward control effectively erase the frequency correlation of photon pairs. Moreover, we implement the Hong–Ou–Mandel interference between the spectrally multiplexed single photons and photons from an independent weak coherence source, which indicates that the multiplexed single photons are highly indistinguishable after the spectral manipulation. Our results pave a way for on-chip scalable and high-performance HSPS with spectral multiplexing toward deterministic single-photon emission.