This thesis is devoted to the study of gravitational theories which can be seen as modifications or generalisations of General Relativity. The motivation for considering such theories, stemming from Cosmology, High Energy Physics and Astrophysics is thoroughly discussed (cosmological problems, dark energy and dark matter problems, the lack of success so far in obtaining a successful formulation for Quantum Gravity). The basic principles which a gravitational theory should follow, and their geometrical interpretation, are analysed in a broad perspective which highlights the basic assumptions of General Relativity and suggests possible modifications which might be made...