The attapulgite / natural rubber (NR) micro-nano composites were prepared by co-coagulating rubber latex and clay aqueous suspension. The vulcanization behavior, mechanical properties and microcosmic structure of the composites were investigated. The field emission scanning electron microscope (FESEM) micrographs of the composites showed that the attapulgite stick particles inserted into the rubber. The interaction between the attapulgite and natural rubber could be improved by using the attapulgite pre-modified with cetyltrimethylammonium bromide (CTAB). The properties of the composites filled with CTAB-modified attapulgite are better than that of the composites filled with carbon black N330. The best properties, which the tensile strength, the 300% tensile modulus and the tear strength increase by 46.9%, 269.7%, 102.0%, respectively, compared with the composites with the unmodified attapulgite, can be obtained, when 20 phr CTAB-modified attapulgite was added.