The problem of determining high-accuracy minimum-time Earth-orbit transfers using low-thrust propulsion is considered. The optimal orbital transfer problem is posed as a constrained nonlinear optimal control problem and is solved using a variable-order Legendre-Gauss-Radau quadrature orthogonal collocation method. Initial guesses for the optimal control problem are obtained by solving a sequence of modified optimal control problems where the final true longitude is constrained and the mean square difference between the specified terminal boundary conditions and the computed terminal conditions is minimized. It is found that solutions to the minimumtime low-thrust optimal control problem are only locally optimal, in that the solution has essentially the same number of orbital revolutions as that of the initial guess. A search method is then devised that enables computation of solutions with an even lower cost where the final true longitude is constrained to be different from that obtained in the original locally optimal solution. A numerical optimization study is then performed to determine optimal trajectories and control inputs for a range of initial thrust accelerations and constant specific impulses. The key features of the solutions are then determined, and relationships are obtained between the optimal transfer time and the optimal final true longitude as a function of the initial thrust acceleration and specific impulse. Finally, a detailed postoptimality analysis is performed to verify the close proximity of the numerical solutions to the true optimal solution. Nomenclature a = semimajor axis, m e = eccentricity f = second modified equinoctial element g = third modified equinoctial element g e = sea-level acceleration due to Earth gravity, m∕s 2 H = optimal control augmented Hamiltonian h = second modified equinoctial element i = inclination, deg or rad (i r , i θ , i h ) = rotating radial coordinate system J 2 = second zonal harmonic J 3 = third zonal harmonic J 4 = fourth zonal harmonic k = fifth modified equinoctial element L = sixth modified equinoctial element (true longitude), rad or deg m = mass, kg n = mean motion P k = Legendre polynomial of degree k p = first modified equinoctial element (semiparameter), m R e = radius of the Earth, m T = thrust, N t = time, s or day u = control direction u h = normal component of control u r = radial component of control u θ = tangential component of control Δ = spacecraft specific force, m · s −2 λ = optimal control costate μ = optimal control path constraint Lagrange multiplier μ e = Earth gravitational parameter, m 3 · s −2 ν = true anomaly, deg or rad Ω = longitude of ascending node, deg or rad ω = argument of periapsis, deg or rad