Herein, the synthesis and characterization methods of natural deep eutectic solvents based on monoterpenoids have been presented. Low viscous fluids with suitable physicochemical properties are produced. The materials are non-toxic, biodegradable, and cost-effective. Thus, they can be used to develop sustainable solvents for various processes and can find their applications in various fields. A theoretical study based on quantum chemistry and classical molecular dynamics is used for the nanoscopic characterization of structure, dynamics, and hydrogen bonding. The reported results help analyze the properties of this new family of solvents. The required information for developing structure–property relationships for proper solvent design to form a sustainable chemistry framework is obtained.

This work was funded by the Junta de Castilla y Leon (Spain, project NANOCOMP-BU058P20 ) and the Ministerio de Ciencia, Innovación y Universidades (Spain, project RTI2018–101987-B-I00 ).