Increasing the dimensionality of quantum entanglement is a key enabler for high-capacity quantum communications and key distribution [1, 2], quantum computation [3] and information processing [4, 5], imaging [6], and enhanced quantum phase measurement [7,8]. A large Hilbert space can be achieved through entanglement in more than one degree of freedom (known as hyperentanglement [2,7,9]), where each degree of freedom can also be expanded to more than two dimensions (known as high-dimensional entanglement). The high-dimensional entanglement can be prepared in several physical attributes, for example, in orbital angular momentum [1,[10][11][12] and other spatial modes [13][14][15]. The drawback of these high-dimensional spatial states is complicated beam-shaping for entanglement generation and detection, which reduces the brightness of the sources as the dimension scales up, and complicates their use in optical-fiber-based communications systems. In contrast, the continuous-variable energy-time entanglement [16][17][18][19][20][21][22] is intrinsically suitable for high-dimensional coding and, if successful, can potentially be generated and be communicated in the telecommunication network. However, most studies focus on time-bin entanglement, which is discrete-variable entanglement with typical dimensionality of two [23][24][25]. Difficulties in pump-pulse shaping and phase control limit the dimensionality of the time-bin entanglement [26], and high-dimensional time-bin entanglement has not been fully characterized because of the overwhelmingly complicated analyzing interferometers. On the other hand, a biphoton state with a comb-like spectrum could potentially serve for high-dimensional entanglement generation and take full advantage of the continuous-variable energy-time subspace. Based on this state, promising applications have been proposed for quantum computing, secure wavelength-division multiplexing, and dense quantum key distribution [3,27,28]. A phase-coherent biphoton frequency comb (BFC) is also known for 3 its mode-locked behavior in its second-order correlation. Unlike classical frequency combs, where mode-locking directly relies on phase coherence over individual comb lines, the mode-locked behavior of a BFC is the representation of the phase coherence of a biphoton wavepacket over comb-line pairs, and results in periodic recurrent correlation at different time-bins [29, 30]. This time correlation feature can be characterized through quantum interference when passing the BFC through an unbalanced Hong-Ou-Mandel (HOM)-type interferometer [31]. A surprising revival of the correlation dips can be observed at time-bins with half the period of the BFC revival time.However, because of the limited type-I collinear spontaneous parametric downconversion (SPDC) configuration in the prior studies [29], post-selection was necessary for the BFC generation where the signal and idler photons are indistinguishable, limiting the maximum two-photon interference to 50 %.Here we achieve high-dimensional hyperentangle...