The nuclear hyperfine structure of anomalous muonium in GaP has been r
esolved using muon level-crossing resonance. We find that 43% of the u
npaired electron spin density resides on the nearest-neighbor Ga and 3
5% on the nearest-neighbor P on the [111] axis of symmetry. The s and
p character of the unpaired spin density indicates that the Ga and P a
re displaced 0.23 and 0.54 angstrom away from the bond center. The now
complete set of measured muon and nearest-neighbor nuclear hyperfine
parameters for anomalous muonium in GaP and GaAs allows a detailed com
parison of the two compounds, showing that the distribution of spin de
nsity among the group-III and group-V nearest neighbors in GaP is almo
st exactly the opposite of that in GaAs. This is contrary to what one
would expect from a simple model of anomalous muonium in compound semi
conductors involving an account of bonding characteristics.