Two couples of enantiomeric pinene-containing N^C^N and C^N^N-coordinated Pt(II) isocyanide complexes decorated with long alkyl chains have been prepared and characterized. Complexes (−)- 1 and (−)- 2 form chiral ordered self-assemblies through Pt⋅⋅⋅Pt, π − π , and hydrophobic-hydrophobic interactions in nonpolar solvents, which is manifested by scanning electron and confocal microscope studies. Complexes (−)- 1 and (−)- 2 display appreciable aggregation-induced emission enhancement behavior in the CH 2 Cl 2 / n -hexane system with the emission quantum yield (Φ em) intensified by a factor of twenty. The complexes exhibit thermo-responsive sol-to-gel transition and solvent-tuned emission colors in higher alcohols or alkane solvents. Considerable circularly polarized luminescence (CPL) signals deriving from chiroptically active 3MMLCT transition with the g lum value of 10−2 order have been found for most sols at RT. Despite minor structural variations in complexes (−)- 1 and (−)- 2 , the CPL activity of Pt(N^C^N) isocyanide complex (−)- 1 is more sensitive to solvent and temperature. In contrast, the CPL activity of Pt(N^N^C) isocyanide complex (−)- 2 is inert to external factors. This research provides a new design strategy for developing tunable CPL platinum(II) complex sol-gels. [Display omitted] • Two couples of Pt(II) isocyanide complexes decorated with long alkyl chains have been prepared. • Sol-gels have been generated in nonpolar solvents. • All complexes exhibit prominent aggregation-induced enhancement of emission. • Minor structural variations lead to different tunabilities on circularly polarized luminescence. [ABSTRACT FROM AUTHOR]