Since their discovery, over the years, molecular gels have been constantly drawing the attention of chemists from various scientific fields. Their structural softness together with the orderliness at the molecular level provides such molecules immense potential for the amplification of their properties. Using this chemistry, one can easily realize a macroscopic outcome from a molecular level modulation. This phenomenon is governed by the principle of supramolecular interactions that introduce a unique “reversibility” to the system. The new generation of gel chemistry is now tending more towards the development of new attractive functions to create smart materials for achieving outstanding response or unprecedented selectivity over a process. However, for the successful implementation of this mission, it is really essential to correlate gel functions with their structures. This focus review is an attempt to find such a correlation, which can motivate and stimulate this existing field towards precisely designing molecular gels for the desired functions.