The present disclosure provides a LED package structure and a LED light-emitting device. The LED package structure comprises a LED chip and a wavelength converting layer covering the LED chip. The wavelength converting layer contains red phosphor, which has lower amount in edge portion than in center portion. It is possible to avoid direct or indirect excitation for generating red light in edge portion of the LED chip by adjusting the amount of red phosphor in edge portion to be lower, so that the color temperature in edge portion may be adjusted toward to high color temperature, and thus the phenomenon of yellow halo may be alleviated.