The binding energy spectra (BES) of valence shells of CH2BrCl and CF2BrCI have been measured at a series of different azimuthal angles by an (e, 2e) electron momentum spectrometer employing noncoplanar symmetric geometry at an impact energy of 1200 eV plus binding energy. The experimental momentum profiles (XMPs) are extracted from the sequential BES and compared with the theoretical ones calculated by using Hartree-Fock (HF) and density functional theory (DFr-B3LYP) calculations with 6-311G, 6-311++G**, and aug-cc-pVTZ basis sets. In general, the DFT-B3LYP calculations using the larger basis sets 6-311++G** and aug-cc-pVTZ describe the XMPs well for both molecules. Moreover, the pole strengths of main ionizations from the inner valence orbitals 2a', 3a', and 1a' of CH2BrCl are determined, and the controversial ordering of two outer valence orbitals 3a '' and 6a' of CF2BrCl has also been assigned unambiguously.