tunable energy range. [1][2][3][4] Among the emerging natural hyperbolic materials, a particular interest has been focused on orthorhombic-phase molybdenum trioxide (α-MoO 3 ) for sustaining extremely anisotropic HPhPs in the mid-IR range, which also provides multiple photonic operation routes such as the layer-twisting, [5][6][7][8] heterojunction, [9] artificial structure, [10][11][12][13][14][15] doping, [16,17] and ambient dielectric modulation. [11,18,19] These highly anisotropic HPhPs of α-MoO 3 stem from three socalled Reststrahlen bands (RBs) with opposite-signed refractive indices along the three principal crystal orientations in the mid-IR range, which results from the strong anisotropic structure. [2,3,20] The spectral energy in RB1 (545-850 cm −1 ) and RB2 (820-972 cm −1 ) supports in-plane hyperbolic polaritonic modes (along [001] and [100], respectively), while RB3 (958 to 1010 cm −1 ) sustains the in-plane elliptic polaritonic modes (Figure S1, Supporting Information). [3] To date, the investigations on the HPhP launching and propagating in α-MoO 3 have predominately been limited to photon wavenumbers in the range of 900-1010 cm −1 (9.9-11.1 µm) through scattering-type scanning near-field optical microscopy (s-SNOM), which covers RB3 and the upper part of RB2. Few spectral studies based on nano-FTIR have extended to the mid-IR transverse optical (TO) phonon frequency of RB2 (820 cm −1 ) using a broadband source, and the nano-imaging studies in this spectral range usually need to be reconstructed from the hyperspectral data. [2,10,21] Two possible reasons make it challenging to study HPhPs in this spectral band through s-SNOM. First, a polarized and high-power narrowband laser source in this mid-IR range (like the free-electron laser [22] ), or a broadband mid-IR radiation (like synchrotron source [21,23,24] ), is not readily accessible, which is essential to obtain a highquality near-field optical nano-image. [25][26][27][28] Second, the inherent damping rate of HPhPs in α-MoO 3 dramatically increases toward the TO phonon frequencies at 820 cm −1 (the lower band edge of RB2), which hinders the observation of HPhPs in this range. [1,3,12] Alternatively, Gao et al. employed an electron beam instead of a light source through electron energy loss spectroscopy (EELS) to investigate HPhPs in a large energy range that covers all three full RBs in mid-IR. [4] However, this nonoptical technique has a short penetration depth and a low spectral energy resolution limit. [4] The in-plane anisotropic HPhPs properties, especially in the spectral range that covers both RB1 Anisotropic hyperbolic phonon-polaritons (HPhPs) in a van der Waals material, orthorhombic-phase molybdenum trioxide (α-MoO 3 ), provide strategies in multiple dimensions to manipulate photons at the nanoscale. However, the nano-imaging studies of the in-plane HPhPs along orthogonal crystal orientations are still rare. In this work, the launching and propagating properties of HPhPs are studied in α-MoO 3 upon a holey silicon nitride microcavity ...