We report the first magneto-caloric and calorimetric observations of a magnetic-field-induced phase transition within a superconducting state to the long-sought exotic "FFLO" superconducting state first predicted over 50 years ago. Through the combination of bulk thermodynamic calorimetric and magnetocaloric measurements in the organic superconductor κ -(BEDT-TTF)2Cu(NCS)2, as a function of temperature, magnetic field strength, and magnetic field orientation, we establish for the first time that this field-induced first-order phase transition at the paramagnetic limit Hp for traditional superconductivity is to a higher entropy superconducting phase uniquely characteristic of the FFLO state. We also establish that this high-field superconducting state displays the bulk paramagnetic ordering of spin domains required of the FFLO state. These results rule out the alternate possibility of spin-density wave (SDW) ordering in the high field superconducting phase. The phase diagram determined from our measurements -including the observation of a phase transition into the FFLO phase at Hp -is in good agreement with recent NMR results and our own earlier tunnel-diode magnetic penetration depth experiments, but is in disagreement with the only previous calorimetric report. 74.25.Dw, 74.70.Kn, 74.25.Ha Magnetic fields destroy superconductivity. In most cases, this occurs due to the formation of magnetic vortices -non-superconducting regions containing a magnetic field flux line shielded by circulating electrons -which increase in density as the magnetic field strength increases, ultimately displacing the superconducting phase. In the absence of magnetic vortices, the paramagnetic spin susceptibility of the electrons making up the superconducting "Cooper pairs" places another upper limit on superconductivity in magnetic fields. Because the electrons in these pairs have oppositely aligned magnetic moments (spins), the reduction in magnetic energy due to flipping the spin of an individual electron will exceed the reduction in electronic energy available from the formation of the Cooper pairs above a critical magnetic field H P known as the Clogston-Chandrasakar paramagnetic limit [1,2]. A phase transition from the superconducting to the normal metallic state is therefore expected at H P . Some 50 years ago, however, Fulde and Ferrell [3] and Larkin and Ovchinnikov [4] predicted that there might instead be a phase transition at H P to a different superconducting phase in which paramagnetic spin domains coexist with a spatially inhomogeneous superconducting phase. This "FFLO state" is expected to exist at fields above H P in electronically clean, anisotropic superconducting materials [5][6][7].The search for inhomogeneous superconductivity has spanned many years, and began in low dimensional single layers of superconducting materials [8]. The first clear calorimetric observations of a bulk field induced phase transition between two superconducting phases were observed in the heavy fermion compound CeCoIn 5 [9,10]. This tran...