The development of new applications of nanofluids in chemical engineering and other technologies has stimulated significant interest in computational simulations. Motivated by coating applications of nanomaterials, we investigate the transient nanofluid flow from a time-dependent spinning sphere using laminar boundary layer theory. The free stream velocity varies continuously with time. The unsteady conservations equations are normalized with appropriate similarity transformations and rendered into a ninth-order system of nonlinear coupled, multidegree ordinary differential equations. The transformed nonlinear boundary value problem is solved using the homotopy analysis method (HAM), a semicomputational procedure achieving fast convergence. Computations are verified with an Adomian decomposition method (ADM). The influence of acceleration parameter, rotational body force parameter, Brownian motion number, thermophoresis number, Lewis number, and Prandtl number on surface shear stress, heat, and mass (nanoparticle volume fraction) transfer rates is evaluated. The influence on boundary layer behavior is also investigated. HAM demonstrates excellent stability and leads to highly accurate solutions.