The experimental electron density study of Ti(C5H4Me)(2)[(CH2)(2)CMe2] provides direct evidence for the presence of (C-C)-> Ti agostic interactions. In accord with the model of Scherer and McGrady, the C-alpha-C-beta bond densities no longer show cylindrical symmetry in the vicinity of the Ti atom and differ markedly from those of the other C-C bonds. At the points along the C-alpha-C-beta bond where the deviation is maximal the electron density is elongated toward the metal center. The distortion is supported by parallel theoretical calculations. A calculation on an Mo complex in which the agostic interaction is absent supports the Scherer and McGrady criterion for agostic interactions. Despite the formal d(0) electron configuration for this Ti(IV) species, a significant nonzero population is observed for the d orbitals, the d orbital population is largest for the d(xy) orbital, the lobes of which point toward the two C-alpha atoms. Of the three different basis sets for the Ti atom used in theoretical calculations with the B3LYP functional, only the 6-311++G** set for Ti agrees well with the experimental charge density distribution in the Ti-(C-alpha-C-beta)(2) plane.