On the basis of tactile interactions, this study aims to capture and analyze users' imaginations on materials. This research also proposes an 'unexpected' new tactile material for design from the viewpoint of tactile interactions. To capture imaginations, we investigated users' tactile interactions in an experiment. The experiment used samples of six common natural and artificial materials, along with the proposed new micro-print-based material. A concept network-based method was employed in two stages to analyze the experimentally obtained verbalized protocols and to identify induced imaginations. This method allowed us to capture and analyze the inexplicit imaginations and associative concepts behind the verbalized protocols. This research found that the feel of materials' tactile naturalness and users' preference to the tested samples are related to their inexplicit imaginations and the complexity of their concept networks. The imagination and concept network of the proposed micro-print material are distinct and different from the existing natural or artificial materials. These findings will provide the basis for employing new analysis tools and facilitate the development of unexpected tactile materials which will enhance the creative ideas for design.