The structures, C-H stretching frequencies, and dipole moments of HCN-Cu-n ( n = 1-3) clusters are determined through high-resolution infrared spectroscopy. The complexes are formed and probed within superfluid helium droplets, whereby the helium droplet beam is passed over a resistively heated crucible containing copper shot and then through a gas HCN pickup cell. All complexes are found to be bound to the nitrogen end of the HCN molecule and on the "atop site" of the copper cluster. Through the experimental C-H vibrational shifts of HCN-Cu-n and ab initio calculations, it was found that the HCN-metal interaction changes from a strong van der Waals bond in n = 1 to a partially covalent bond in HCN-Cu-3. Comparisons with existing infrared data on copper surfaces show that the HCN-Cu-n bond must begin to weaken at very large copper cluster sizes, eventually returning to a van der Waals bond in the bulk copper surface case.