A least-squares–based optimization and reconstruction algorithm has been developed for rapid metabolic imaging in the context of hyperpolarized 13C. The algorithm uses a priori knowledge of resonance frequencies, J-coupling constants, and T2* values to enable acquisition of high-quality metabolic images with imaging times of approximately 100 ms for an 8-cm field of view (FOV) and 0.5 cm isotropic resolution. A root-mean-square error (rMSE) analysis is introduced to optimize metabolic image quality by appropriate choice of pulse sequence parameters, echo times, and signal model. By performing the reconstruction in k-space, the algorithm also allows the inclusion of the effect of chemical shift evolution during the readout period. Single-interleaf multiecho spiral chemical shift imaging (spCSI) is analyzed in detail as an illustrative example for the use of the new reconstruction and optimization algorithm. Simulation of the in vivo spectrum following the bolus injection of hyperpolarized 13C1 pyruvate shows that single-interleaf spiral spectroscopic imaging can achieve image quality in 100 ms, comparable to the performance of a 13-s phase-encoded chemical shift imaging (FIDCSI) experiment. Single-interleaf spCSI was also tested at a 3-T MR scanner using a phantom containing approximately 0.5-M solutions of alanine, lactate, and a pyruvate-pyruvate hydrate C1-C2 ester at thermal equilibrium polarization, all enriched to 99% 13C in the C1 carbonyl positions. Upon reconstruction using the k-space–based least-squares technique, metabolite ratios obtained using the spCSI method were comparable to those obtained using a reference FIDCSI acquisition. Magn Reson Med 58:245–252, 2007. © 2007 Wiley-Liss, Inc.