Puzzling multiferroic behavior observed recently in spin-1/2 one-dimensional chain cuprate LiCu 2 O 2 with edge-shared arrangement of CuO 4 plaquettes and incommensurate spiral spin ordering is consistently explained to be a result of the nonrelativistic exchange-induced electric polarization on the Cu 2+ centers substituting for the positions native for the Cu 1+ ions. These substituent centers are proven to be an effective probe of the spin incommensurability and magnetic field effects.Intensive study of magnetoelectric and multiferroic materials is stimulated both by their potential application in novel technological devices and growing interest to fundamental problems of magnetoelectric coupling which proved to be a very sensitive tool to uncover subtle details of interrelation between charge, orbital, and spin ordering. However, due to its complexity, theoretical understanding of the mechanism͑s͒ of strong magnetoelectric coupling is far from being satisfactory. Remarkable demonstration of the present day situation is provided by a hot discussion around recent observations of multiferroic behavior concomitant the incommensurate spin spiral ordering in chain cuprates LiCuVO 4 ͑Refs. 1-3͒ and LiCu 2 O 2 ͑Ref. 4͒ challenging the multiferroic community. At first sight, these cuprates seem to be prototypical examples of 1D spiral-magnetic ferroelectrics revealing the relativistic mechanism of "ferroelectricity caused by spin-currents 5 " with the textbook expression for the uniform polarization induced by a spin spiral with the wave vector Q: P ϰ ͓e 3 ϫ Q͔, where e 3 is a vector orthogonal to the spin spiral plane 6 or P ij ϰ [R ij ϫ ͓S i ϫ S j ͔], where R ij denotes the vector connecting the two sites and ͓S i ϫ S j ͔ is a local spin current. 5 However, both systems reveal a mysterious behavior with conflicting results obtained by different groups. Indeed, Yasui et al. 2 claim the LiCuVO 4 reveals clear deviations from the predictions of spin-current models 5,6 while Schrettle et al. 3 assure its applicability. In contrast to LiCuVO 4 , the LiCu 2 O 2 shows up a behavior which is obviously counterintuitive within the framework of spiralmagnetic ferroelectricity. 4 It is worth noting that at variance with Park et al., 4 Naito et al. 1 have not found any evidence for ferroelectric anomalies in LiCu 2 O 2 . Such a discrepancy one observes in microscopic model approaches as well. The relativistic LSDA calculations 7 seemingly explain the LiCuVO 4 data 3 but fail in case of LiCu 2 O 2 . However, a detailed analysis of relativistic effects for the system of e g holes in a perfect chain structure of edge-shared CuO 4 plaquettes as in LiCuVO 4 and LiCu 2 O 2 shows that the in-chain spin current does not produce an electric polarization because of an exact cancellation of two Cu-O-Cu paths. 8 Moreover, recently we have shown 9 that the multiferroicity in LiCuVO 4 may have nothing to do with relativistic effects and can be consistently explained, if the nonrelativistic exchangeinduced electric polarization on the out-of-c...