Hybrid composites with great potential for white light LED and temperature sensing obtained through a simple, low cost, and environmental benign way is highly desirable and remains a challengeable task. Herein we present luminescent hybrid composites both in the form of powder and transparent film by simply mixing organic sensitizer, aminoclay (AC), and lanthanide (Ln(3+)) in aqueous solution, the emission color of which can be fine-tuned by changing various parameters such as the molar ratio of Eu(3+) to Tb(3+), excitation wavelength, and the temperature. White lights with satisfied color coordinates have been achieved. The emission intensity ratio of (5)D4 → (7)F5 transition (Tb(3+)) to (5)D0 → (7)F2 transition (Eu(3+)) of the composite containing both Eu(3+) and Tb(3+) can be linearly related to temperature in the range from 78 K to 288 K. These characteristics make the composites suitable for optoelectronic devices such as thermosensors and white light LED.