We have investigated the photodissociation spectroscopy of the Al+-acetaldehyde bimolecular complex over the spectral range 212-345 nm. We find evidence for three overlapping molecular absorption bands in the near UV. Two of the bands are unstructured and are assigned as 1A(") and 2A"<--1A'. These continuum bands are of mixed character with contributions from Al+-centered 3pπ(A")<--3ssigma(A'), acetaldehyde-centered pi(*)(A")<--n(A'), and Al-acetaldehyde charge transfer excitation processes. The third absorption band at short wavelengths, λ>223 nm, shows a prominent vibrational progression with a mode frequency omega(e)=210+/-4 cm(-1). The structured band is assigned as 2A'<--1A' and correlates to an Al+-centered 3pπ(A')<--3ssigma(A') radiative transition; the vibrational progression is assigned to the intermolecular Al+-acetaldehyde in-plane bend. Spectroscopic results are in good agreement with ab initio predictions.