We report on Fermi Large Area Telescope (LAT) and multi-wavelength results on the recently-discovered very-high-energy (VHE, $E>$ 100 GeV) blazar S4 0954+65 ($z=0.368$) during an exceptionally bright optical flare in 2015 February. During the time period (2015 February, 13/14, or MJD 57067) when the MAGIC telescope detected VHE $gamma$-ray emission from the source, the Fermi-LAT data indicated a significant spectral hardening at GeV energies, with a power-law photon index of $1.8 pm 0.1$---compared with the 3FGL value (averaged over four years of observation) of $2.34 pm 0.04$. In contrast, Swift/XRT data showed a softening of the X-ray spectrum, with a photon index of $1.72 pm 0.08$ (compared with $1.38 pm 0.03$ averaged during the flare from MJD 57066 to 57077), possibly indicating a modest contribution of synchrotron photons by the highest-energy electrons superposed on the inverse Compton component. Fitting of the quasi-simultaneous ($<1$ day) broadband spectrum with a one-zone synchrotron plus inverse-Compton model revealed that GeV/TeV emission could be produced by inverse-Compton scattering of external photons from the dust torus. We emphasize that a flaring blazar showing high flux of $gtrsim 1.0 times 10^{-6}$ photons cm$^{-2}$ s$^{-1}$ ($E>$ 100 MeV) and a hard spectral index of $Gamma_{rm GeV} < 2.0$ detected by Fermi-LAT on daily time scales is a promising target for TeV follow-up by ground-based Cherenkov telescopes to discover high-redshift blazars, investigate their temporal variability and spectral features in the VHE band, and also constrain the intensity of the extragalactic background light.
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