Photometric and spectroscopic analysis of high galactic latitude molecular clouds. II - High-resolution spectroscopic observations of NA I, CA II, CA I, CH, and CH(+1) High-resolution spectroscopic observations in the wavelengths of thespecies Na I, Ca II, and Ca I and the molecular species CH and CH(+)have been performed toward stars behind a variety of high galacticlatitude molecular clouds (HLCs). Seventeen new detections of molecularabsorption are reported. The sizes, densities, and molecular contentfound for the HLCs are consistent with an interpretation of HLCmolecular cores as extremely compact structures of enhanced molecularcontent which may have evolved from larger H I shells.