Increasing carbon dioxide accumulation in earth's atmosphere and the depletion of fossil resources pose huge challenges for our society and, in particular, for all stakeholders in the transportation sector. The Cluster of Excellence 'Tailor-Made Fuels from Biomass' at RWTH Aachen University establishes innovative and sustainable processes for the conversion of whole plants into molecularly well-defined fuels exhibiting tailored properties for low-temperature combustion engine processes, enabling high efficiency and low pollutant emissions. The concept of fuel design, that is, considering fuel's molecular structure to be a design degree of freedom, aims for the simultaneous optimisation of fuel production and combustion systems. In the present contribution, three examples of tailor-made biofuels are presented. For spark ignition engines, both 2-methylfuran and 2-butanone show increased knock resistance compared to RON95 gasoline, thus enabling a higher compression ratio and an efficiency gain of up to 20% at full-load operation. Moreover, both fuels comprise a good mixture formation superior to the one of ethanol, especially under difficult boundary conditions. For compression ignition engines, 1-octanol enables a remarkable reduction in engine-out soot emissions compared to standard diesel fuel due to the high oxygen content and lower reactivity. This advantage is achieved without sacrificing the high indicated efficiency and low NO X emissions.