We have determined the magnetic properties of single-crystalline Au nanorods in solution using an optically detected magnetic alignment technique. The rods exhibit a large anisotropy in the magnetic volume susceptibility (Á V ). Á V increases with decreasing rod size and increasing aspect ratio and corresponds to an average volume susceptibility ( V ), which is drastically enhanced relative to bulk Au. This high value of V is confirmed by SQUID magnetometry and is temperature independent (between 5 and 300 K). Given this peculiar size, shape, and temperature dependence, we speculate that the enhanced V is the result of orbital magnetism due to mesoscopic electron trajectories within the nanorods. DOI: 10.1103/PhysRevLett.111.127202 PACS numbers: 75.75.Àc, 73.22.Àf, 75.20.En, 78.67.Qa Bulk Au is a diamagnetic material, i.e., one with a negative volume magnetic susceptibility Au . Recently, it was reported that Au nanoparticles (NPs), with functionalized surfaces, show a broad range of magnetic behavior, ranging from (enhanced) diamagnetic [1,2] to (super)paramagnetic [3][4][5] and even ferromagnetic up to room temperature [6,7]. The NP size and the type of capping molecules, strongly binding to or weakly interacting with Au, appear to influence the magnetic response. Several explanations were suggested, such as competing magnetic contributions of the NP core and surface [3], the formation of a magnetic moment due to the exchange of charges at the Au-ligand interface [5,6,8], the creation of large orbital moments due to electron motion within surface clusters [9], and the occurrence of persistent currents in the Au core [2]. However, so far, the origin of this unexpected magnetism and why it differs strongly between different types of NPs is not yet understood [2,10,11].We employ a novel magnetic alignment technique to measure the magnetic properties of rod-shaped Au NPs in solution. We focus on relatively large NPs (all dimensions >7 nm) that are single crystalline. The degree of alignment is measured optically, through the magnetic field-induced linear dichroism and birefringence, across the Au surface plasmon resonance (SPR) that arises due to collective oscillation modes of the conduction electrons [12,13]. We find an enhanced (dia)magnetic behavior, which does not depend on temperature (in the range 5-300 K). We speculate that this enhanced magnetism is an orbital effect, resulting from mesoscopic electron trajectories within the NPs [2,14].The optically detected magnetic alignment technique relies on the anisotropy of both the optical and magnetic properties of the Au nanorods. Because of their shape, the rods exhibit an anisotropic optical response, determined by their longitudinal ( k ) and transverse ( ? ) polarizabilities [15]. Polarized light, therefore, provides a sensitive tool to determine the alignment of rods [16][17][18][19]. In this Letter, rod alignment is induced by a magnetic field (B) because of the difference in the magnetic susceptibility parallel ( k ) and perpendicular ( ? ) to the lo...