We report two schemes to generate perfect anisotropy in the photoelectron angular 
distribution of a randomly oriented ensemble of polyatomic molecules. In order to exert full 
control over the anisotropy of photoelectron emission, we exploit interferences between 
single-photon pathways and a manifold of resonantly enhanced two-photon pathways. These 
are shown to outperform nonsequential (w,2w) bichromatic phase control for the example of 
CHFClBr molecules. We are able to optimize pulses that yield anisotropic photoelectron 
emission thanks to a very efficient calculation of photoelectron momentum distributions. 
This is accomplished by combining elements of quantum chemistry, variational scattering 
theory, and time-dependent perturbation theory.