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In this study, a series of A-site strontium-doped La_1-xSr_xCeO_3-δ (x = 0.2, 0.4, 0.6, 0.8) perovskite catalysts were synthesized via the ethylenediaminetetraacetic acid (EDTA) sol-gel method for hydrogen production by methanol steam reforming. The fresh and the reduced catalysts are characterized by scanning X-ray (XRD), energy dispersive X-ray spectroscopy (EDS) and scanning electron microscopy (SEM) techniques. Results showed that La_0.6Sr_0.4CeO_3-δ exhibited the best performance among the La_1-xSr_xCeO_3-δ catalysts. The operating parameters were optimized to study the catalytic performance of La_0.6Sr_0.4CeO_3-δ, including catalytic temperature, water–methanol ratio (W/M) and liquid hourly space velocity (LHSV). However, the excessive strontium content led to a decrease in hydrogen production amount per unit time, and the high W/M promoted the reverse water–gas shift reaction (RWGS), which resulted in a decrease in CO selectivity and an increase in CO₂ selectivity. In addition, the optimal reaction parameters are as follows: reforming temperature of 700 °C; W/M of 3:1; LHSV of 20 h⁻¹. Furthermore, the methanol conversion rate of La_0.6Sr_0.4CeO_3-δ can reach approximately 82%, the hydrogen production can reach approximately 3.26 × 10⁻³ mol/g_(cat)/min under the optimum reaction conditions. Furthermore, La_0.6Sr_0.4CeO_3-δ exhibits high hydrogen selectivity (85%), which is a promising catalyst for MSR application.