A L-glutamide attached terpyridine (G-tpy) enhanced lanthanide supramolecular assembly (G-tpy+Ln3+) (Ln3+ = Eu3+ and Tb3+) was fabricated in a facile but efficient way in a mixed solvent of cyclohexane-ethanol (9:1). Significantly, the resultant fibrous assembly could show remarkable enhancement through coordination-driven secondary chirality of molecular gels at 1:1 stichometry of G-tpy+Ln3+ ratio. Furthermore, this system showed high fluorescence quantum yield of 25.5% and 32.7% with Eu3+ and Tb3+ in cyclohexane-ethanol. This type of G-tpy+Ln3+ self-assembly can be inherently applicable in sensing or bioimaging technology because of their multiple-stimuli responsive behaviour.