The development of advanced nonlinear media as well as active optical materials for light conversion applications is an ongoing process. [1,2] Aims include improved conversion efficiencies, brilliance, i.e., beam quality, and accessible target wavelengths. Light-converting materials for white-light generation are of particular interest, e.g., for white light-emitting diodes (LEDs) and their applications. Here, phosphors offer great efficiency even at low driving power densities and huge spectral versatility across the visible spectrum. [3][4][5][6] The virtually perfect Lambertian angular emission pattern of such functionalized LEDs is highly desirable in applications such as backlights in displays, while others require low-étendue sources with limited angular spread. [7,8] Laser-driven phosphors in automotive headlights are a recent, prominent example where a small laser spot is exploited to achieve a virtual point source and tailorThe vast optical nonlinearity of 1,3,5,7-tetraphenyladamantane (AdPh 4 ) enables efficient frequency conversion. The observed spectrum depends heavily on the material's habitus. In particular, it shows nonlinear white-light generation when its powder form is irradiated in the near-infrared, similar to an analogous organotin sulfide cluster [(PhSn) 4 S 6 ]. In contrast, single crystals of AdPh 4 exclusively exhibit narrow-band second-harmonic generation, i.e., discrete conversion within the crystal, rather than spectrally broadband white-light emission. This shows that crystallinity restricts the nonlinear response to the symmetryallowed higher-harmonics, in this case the even-numbered, second harmonic, and inhibits the quasi-continuum white-light emission. Using the diamondoidbased material significantly enhances compatibility with conventional production techniques using photorefractive polymers and is thus an important step towards the fabrication of all-integrated white-light emitting devices.