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Systematic powder diffraction studies have been carried out to establish the magnetic phase diagram of La2−2xSr1+2xMn2O7 (LSMO327) in a wide hall concentration range (0.30 ≤ x ≤ 0.50), using the HERMES diffractometer. LSMO327 exhibits a planar ferromagnetic structure for 0.32 ≤ x ≤ 0.38 at low temperatures. A finite canting angle between planar magnetic moments on neighboring planes starts appearing around x ∼ 0.40 and reaches 180• (A-type antiferromagnet) at x = 0.48. At x = 0.30, on the other hand, the magnetic moments are aligned parallel to the c-axis.