A pharmaceutical composition for treating headache, prepared from eleven Chinese herbal medicines: Chinese angelica root, ligusticum chuanxiong, radix paeoniae lactiflorae, prepared rhizome of rehmannia, uncaria tomentosa, leatherleaf milletia, prunella vulgaris, sicklesenna seed, pearl shell, corydalis tuber, and asarum, and a proper amount of adjuvant materials. A preparation method of the pharmaceutical composition, and uses thereof in the preparation of drugs for treating various headaches, traumatic cranial nerve syndrome, dizziness and vertigo, vexation and irritability, insomnia and dreaminess.