The light-emitting diode (LED) has been the subject of much interest in the role of a backlight module for liquid crystal displays (LCDs). However, a traditional LED lamp is a point-light source, and so is not suitable for use in large LCD panels. This study presents a new packaging method for LEDs, which uses a gapless dual-curvature microlens array (GDMLA) to improve its ability to illuminate a panel. GDMLAs of different dimensions were simulated and fabricated in order to examine their light luminance and uniformity. Commercial optical simulation software, “Tracepro”, was used to obtain a GDMLA of optimized geometry and dimensions. Based on the simulated data, a GDMLA mold was first fabricated using a LIGA-like process (Lithographie Galvanoformung Abformung, LIGA); this was known as the first mold. In this study, the first mold was obtained using a nickel cobalt (Ni–Co) electroplating process. In order to obtain a highly accurate and strong mold, a bulk metallic glass (BMG) alloy, Mg 58Cu 31Y 11, was chosen as the material for the second mold, which exhibits excellent forming ability and high hardness. The pattern of the first mold was replicated onto BMG by hot-embossing, and the shrinkage between the first and the second mold was less than 0.2%. Next, the pattern of the GDMLA on the second mold was replicated onto ultraviolet (UV)-curable resin, producing the final optical film for a LED package. The shrinkage between the second mold and the UV-cured optical film was less than 0.4%; this means that the process exhibits a high replication ability. The fabricated GDMLA had the characteristics of dual curvatures and a high fill-factor of 100%. The light uniformity of the LED package with the GDMLA optical film was measured, and the results demonstrated that the GDMLA is a good optical device for use in LED packages. In addition, the relationship between the simulation and experimental results is assessed and discussed.