Neutron scattering studies of single-crystal LiNiPO4 reveal a spontaneous first-order commensurate-incommensurate magnetic phase transition. Short-and long-range incommensurate phases are intermediate between the high temperature paramagnetic and the low temperature antiferromagnetic phases. The modulated structure has a predominant antiferromagnetic component, giving rise to satellite peaks in the vicinity of the fundamental antiferromagnetic Bragg reflection, and a ferromagnetic component giving rise to peaks at small momentum-transfers around the origin at (0, ±Q, 0). The wavelength of the modulated magnetic structure varies continuously with temperature. It is argued that the incommensurate short-and long-range phases are due to spindimensionality crossover from a continuous to the discrete Ising state. These observations explain the anomalous first-order transition seen in the magnetoelectric effect of this system. . There has been a continuous interest in the spontaneous and magnetic-field induced commensurate-incommensurate magnetic (C-IC) transition over the years [4,5,6]. For instance, in the semimetallic europium tri-arsenide (EuAs 3 ), the ground state of the system is commensurate and as temperature increases the system undergoes a C-IC transition [4]. In copper metaborate, on the other hand, the ground state is incommensurate and undergoes a continuous phase transition to a non-collinear commensurate antiferromagnetic state [7]. It has also been demonstrated that the C-IC transition can be induced by the application of an external magnetic field [5,6].Here, we report a novel C-IC magnetic phase transition in the weakly coupled antiferromagnetic planes of LiNiPO 4 (S=1, Ni 2+ ), its characteristics resemble IC structural phase transitions [8]. LiNiPO 4 is an antiferromagnetic (AF) insulator[9, 10] which belongs to the olivine family of lithium orthophosphates LiMPO 4 (M = Mn, Fe, Co, and Ni) [11]; space group is Pnma[12]. Neutron scattering studies demonstrated that LiMPO 4 (M =Ni, Co) exhibit properties between the two-dimensional (2D) and three-dimensional (3D) with an interlayer coupling that is relatively stronger than the coupling found in the cuprates, for instance [13,14]. These insulators also exhibit a strong linear magnetoelectric (ME) effect, with the observed ME tensor components, α xy , α yx , for LiCoPO 4 and, α xz , α zx , for LiNiPO 4 , in agreement with the antiferromagnetic point groups mmm' and mm'm, respectively, but with some anomalies [15,16,17]. In particular, the ME effect measurements of LiNiPO 4 as a function of temperature reveal a first-order AF transition, and an unusual decrease of the ME coefficient at temperatures below a maximum close to T N [18]. By contrast, the isostructural LiCoPO 4 , LiFePO 4 , and LiMnPO 4 exhibit continuous change of the ME coefficients, indicative of second-order transitions [15]. Magnetic susceptibility studies of polycrystalline LiNiPO 4 showed a significant deviation from the Curie-Weiss law in a temperature range much higher than T N , and...