Dedicated to the memory of Bernd O. Stratmann -A good friend, colleague and mentor.Abstract. Given an α > 1 and a θ with unbounded continued fraction entries, we characterise new relations between Sturmian subshifts with slope θ with respect to (i) an α-Höder regularity condition of a spectral metric, (ii) level sets defined in terms of the Diophantine properties of θ, and (iii) complexity notions which we call α-repetitive, α-repulsive and α-finite; generalisations of the properties known as linearly repetitive, repulsive and power free, respectively. We show that the level sets relate naturally to (exact) Jarník sets and prove that their Hausdorff dimension is 2/(α + 1).