The commercial success of microalgal systems has to a large extent been restricted due to limited light availability and utilisation. Algae utilize the blue and red spectral regions, large amounts of the incoming light energy fall outside this region and remain unused. The spectral conversion of unusable to usable wavelengths will increase the amount of radiation available for photosynthesis. This study was conducted to determine the optimum organic dye among Lumogen Red (LR), Rhodamine 8G (R8G), and Lumogen Yellow (LY) as spectral converters, providing the best light utilisation efficiency in an algal system. The microalga Chlamydomonas reinhardtii was cultivated in double-jacketed cylindrical photo-bioreactors (PBRs) stimulated using 30% UV-a and 5% UV-b fluorescent tubes. Carbohydrate and lipid contents were produced early in the growth phase, whereas biomass and protein content increased after day 4. The LR dye maintained better photo-stability compared to R8G and LY, which displayed a slight wavelength shift and photo-degradation, respectively. The improved biomass production in the LR-assisted PBR was illustrated by increased Y(II), with decreasing Y(NPQ), total chlorophylls, and carotenoids. Pigment biosynthesis was initially increased and then reduced to compensate for the increased irradiation as a means of photoprotection. Gene expression studies showed that algae grown under LR had a 1.6- and 2.9-fold up-regulation of the RuBisCo gene. The applicability of the dye-based algal system was linked to enhanced growth, lipid, protein, carbohydrate, and pigment productions. Moreover, the environmental, economic, and social aspects of improving microalgal cultivation using dye-based wavelength conversion systems were interlinked to the sustainable development goals.