AbstractHigh-dimensional quantum entanglement is a cornerstone for advanced technology enabling large-scale noise-tolerant quantum systems, fault-tolerant quantum computing, and distributed quantum networks. The recently developed biphoton frequency comb (BFC) provides a powerful platform for high-dimensional quantum information processing in its spectral and temporal quantum modes. Here we propose and generate a singly-filtered high-dimensional BFC via spontaneous parametric down-conversion by spectrally shaping only the signal photons with a Fabry-Pérot cavity. High-dimensional energy-time entanglement is verified through Franson-interference recurrences and temporal correlation with low-jitter detectors. Frequency- and temporal- entanglement of our singly-filtered BFC is then quantified by Schmidt mode decomposition. Subsequently, we distribute the high-dimensional singly-filtered BFC state over a 10 km fiber link with a post-distribution time-bin dimension lower bounded to be at least 168. Our demonstrations of high-dimensional entanglement and entanglement distribution show the singly-filtered quantum frequency comb’s capability for high-efficiency quantum information processing and high-capacity quantum networks.