The paper notebook is the trusty companion of the majority of those who engage in scientific research. In this digital era though, there is pressure to abandon paper in favour of the benefits of digital tools. For many researchers, particularly in academic environments, there are a number of barriers to adopting Electronic Laboratory Notebooks, not least of which are anxieties about their ease of use. Another concern is the impact using these tools may have on the quality of experiment records. In order to design digital tools that support researchers recording scientific experiments it is necessary to understand how researchers work with paper and digital tools, and the impacts different designs may have upon what they record. In this thesis, research is presented on the note-taking and experiment capture behaviour of a range of scientific researchers together with requirements for digital tools obtained from this research. A number of original studies are presented that explore how different techniques for eliciting information from the memories of researchers can be used to capture information of value to the experiment record, with both positive and negative consequences. This thesis also includes an overview of the development of a mobile ELN, designed for use by synthetic chemists, to explore the potential to bridge the gap between desktop ELNs and paper-notebooks. The conclusions of this thesis put forward suggestions as to how digital tools could be enhanced in the future to both support researchers recording scientific experiments and to facilitate the management of research projects.