Langmuir films of members of two homologous series, the 4-n-alkyl-49-cyanobiphenyls (nCB) for n52-14 and trans-4-n-alkyl(49-cyanophenyl)cyclohexanes (PCHn) for n52-12, have been studied by recording surface pressure/area isotherms and by Brewster angle microscopy. It has been found that the compounds with very short chains (n(3) and very long chains (n.12 for nCB, n.10 for PCHn) are unable to form compressible monolayers at the air-water interface. Other members of both series can form stable Langmuir films, but both their rigidity and stability as well as the molecular packing vary with the alkyl chain length. The isotherms and BAM images imply that the organization of the liquid crystal molecules in the films is to some extent correlated with their ability to form corresponding mesophase in the bulk: nematogenic compounds tend to form rounded droplet-like domains, whereas smectogenic compounds tend to form flat domains.