We investigate intermodal forward Brillouin scattering in a solid-core photonic crystal fiber (PCF), demonstrating efficient power conversion between the HE11 and HE21 modes, with a maximum gain coefficient of 21.4 W−1 km−1. By exploring mechanical modes of different symmetries, we observe both polarization-dependent and polarization-independent intermodal Brillouin interaction. Finally, we discuss the role of squeeze film air damping and leakage mechanisms, ultimately critical to the engineering of PCF structures with enhanced interaction between high-order optical modes through flexural mechanical modes.