This thesis reports a number of studies that examines low molecular weight hydrogelators forming through in situ chemical reactions and gel the water in which this reaction occurs. This in situ gelation process has allowed a number of chemical and physical reactions and assembly processes to be investigated. Pathway complexity, an exciting concept within chemical systems has been explored with a multi-reactive hydrazone based gelation system that allows different gels to be formed from a single starting point through navigation of the systems’ energy landscape. This work inspired the development of a large family of imine based gelators that would undergo an effectively irreversible tautomerisation. This allowed exploration and characterisation of the systems’ ability to self-sort and co-assemble, at both the molecular and macroscopic level. One particular imine inspired gelator featured a much slower in situ reaction. This allowed characterisation of its reaction kinetics and demonstrated its autocatalytic behaviour. This thesis highlights the link between the chemical reactions that form the individual gelator molecules and the supramolecular assembly process. By using one to control the other, an in-depth understanding of the presented systems has been developed, allowing for the accurate targeting of desired physical properties
