A multi-loop antenna structure and a hand-held electronic device using the same are provided. The multi-loop antenna structure includes a high-frequency radiating body, a low-frequency radiating body, a feeding connecting part and a grounding connecting part. The feeding connecting part electrically connects one terminal of the high-frequency and the low-frequency radiating body to a feeding point. The grounding connecting part grounds the other terminal of the high-frequency and the low-frequency radiating body. The feeding connecting part forms a first folded loop antenna with the high-frequency radiating body and the grounding connecting part for resonating at a first frequency band. The feeding connecting part forms a second folded loop antenna with the low-frequency radiating body and the grounding connecting part for resonating at a second, a third and a fourth frequency band. The first folded loop antenna and the second folded loop antenna are folded for forming a three-dimensional structure.