Mobile devices (smartphones or tablets) as experimental tools (METs) offer inspiring possibilities for science education, but until now, there has been little research studying this approach. Previous research indicated that METs have positive effects on students’ interest and curiosity. The present investigation focuses on potential cognitive effects of METs using video analyses on tablets to investigate pendulum movements and an instruction that has been used before to study effects of smartphones’ acceleration sensors. In a quasi-experimental repeated-measurement design, a treatment group uses METs (TG, N TG  = 23) and a control group works with traditional experimental tools (CG, N CG  = 28) to study the effects on interest, curiosity, and learning achievement. Moreover, various control variables were taken into account. We suppose that pupils in the TG have a lower extraneous cognitive load and higher learning achievement than those in the CG working with traditional experimental tools. ANCOVAs showed significantly higher levels of learning achievement in the TG (medium effect size). No differences were found for interest, curiosity, or cognitive load. This might be due to a smaller material context provided by tablets, in comparison to smartphones, as more pupils possess and are familiar with smartphones than with tablets. Another reason for the unchanged interest might be the composition of the sample: While previous research showed that especially originally less-interested students profited most from using METs, the current sample contained only specialized courses, i.e., students with a high original interest, for whom the effect of METs on their interest is presumably smaller.