Ground-state Al atoms have been reacted with cyclopropylamine (CpNH2) in an adamantane matrix at 77 K. The four paramagnetic species generated in the reaction have been studied by electron paramagnetic resonance (EPR) spectroscopy and their magnetic parameters extracted from the EPR spectra. The isotropic Al hyperfine interactions (hfis) for these radicals vary from 801 to 962 MHz and are consistent with values previously reported for structurally similar Al-centered radicals. The major species formed in the reaction has a highly anisotropic a tensor indicative of an Al-centered radical with a substantial amount of the unpaired spin density residing in the Al 3p orbital. In addition, there is EPR evidence that the insertion products, CpNH(AlH) and CpAlNH2, are formed in the reaction, suggesting that Al atoms can activate the N-H and C-N bonds of amines. It has been shown that a molecule of CpNH2 coordinates to CpNH(AlH), causing the Al, N and H hfi of the N-H insertion product to decrease. The values of the nuclear hfis calculated for the insertion products, using a density functional theory (DFT) method, are comparable to the experimental values.