This study reports on the anisotropic indentation response of α-titanium. Coarse-grained titanium was characterized by electron backscatter diffraction. Sphero-conical nanoindentation was performed for a number of different crystallographic orientations. The grain size was much larger than the size of the indents to ensure quasi-single-crystal indentation. The hexagonal c-axis was determined to be the hardest direction. Surface topographies of several indents were measured by atomic force microscopy. Analysis of the indent surfaces, following Zambaldi and Raabe (Acta Mater. 58(9), 3516–3530), revealed the orientation-dependent pileup behavior of α-titanium during axisymmetric indentation. Corresponding crystal plasticity finite element (CPFE) simulations predicted the pileup patterns with good accuracy. The constitutive parameters of the CPFE model were identified by a nonlinear optimization procedure, and reproducibly converged toward easy activation of prismatic glide systems. The calculated critical resolved shear stresses were 150 ± 4, 349 ± 10, and 1107 ± 39 MPa for prismatic and basal 〈a〉-glide and pyramidal〈c + a〉-glide, respectively.