The monolayer assemblies incorporating merocyanine J-aggregates, MC(S), MC(Se), 6-Me-MC(S), and their combinations have been fabricated by the Langmuir–Blodgett (LB) technique. At room temperature, absorption and fluorescence spectra of the monolayer assemblies: MC(S), MC(Se), 6-Me-MC(S), are characterized by a sharp J-band and resonance fluorescence. The monolayer assemblies incorporating two dyes: MC(S)/MC(Se), 6-Me-MC(S)/MC(S), 6-Me-MC(S)/MC(Se), bear a single absorption band and accompanying fluorescence band, which are assigned to the homogeneous aggregate of amalgamation type (HA-aggregate). Detailed spectroscopic measurements: absorption spectra in wide temperature range and the fluorescence decay curves, of the MC(S)/MC(Se) assembly have been carried out as a prototype of the HA-aggregate. The continuous shift of the absorption and fluorescence peak positions with increasing x, from x = 0 (MC(S) assembly) to x = 1 (MC(Se) assembly), would indicate that the doping of MC(Se) molecules into the MC(S) J-aggregate does not induce serious structure change. An observation that the fluorescence lifetime of the MC(S)/MC(Se) assembly lies between those of the MC(S) assembly and the MC(Se) assembly implies that the inclusion of MC(Se) molecules does not result in the formation of defect states which may promote non-radiative decay of molecular excitons. The usefulness of the Urbach–Martienssen (UM) rule for the analysis of the low energy tail of absorption spectra of the MC(S)/MC(Se) assembly has been examined.