Organogelation has become an attractive method to generate one-dimensional (1D) nanostructures owing to its simplicity and reproducibility. In select organic solvents, low molecular mass organogelators (LMOGs) form 1D nanostructures by a simple heating and cooling process, which then entangle to form a three-dimensional (3D) network. The solvent molecules are trapped in the 3D network, leading to the formation of a viscoelastic solid. Developing π-conjugated LMOGs has drawn significant attention since these organogelators possess excellent potential in optoelectronic applications such as aggregation-induced emission, field effect transistors, organic solar cells, conducting nanowires, energy transfer, etc. Vigorous research efforts have focused on developing various types of π-LMOGs. In many cases, π-π interactions between flat, large π-cores serve as a driving force for the assembly, with additional intermolecular forces such as van der Waals interactions and hydrogen bonding to enhance the gelation ability. The primary goal of our research is to develop π-LMOGs with tunable electronic properties. Creating new π-LMOGs is nontrivial, however further structural modification of the LMOGs without compromising gelation ability is even more challenging. We have successfully developed novel asymmetrically substituted pyrazine-acene based LMOGs, which allow for controlling both electronic and self-assembling properties. The pyrazine-acene heteroaromatic cores are functionalized with alkyl side groups for solubility and peripheral substituents for electronic property control. In this talk, I will present the effect of type, position, and the number of substituents on the electronic properties. The developed systems exhibited excellent 1D self-assembling properties, including organogelation in select organic solvents. Detailed discussion on the self-assembly properties will also be discussed with various instrumental characterizations.