RE: make the picture a bit larger
Navigate to the Connections : Templates admin page and click the Customize button for the cMap template.
The page will reload with the Customizer on the left and a preview on the right.
Click the back arrow in the upper left of the Customizer and then click the Image panel.
Change the image type to photo, set your desired width, height and crop mode.
Publish the changes.
Take special note of the instructions presented above the directory in the preview.
You will have to follow them in order to customize the display the of single entry profile view of the template.
RE: I would like to maybe attached a CSS file onto the directory. That way I can maybe add a Google font onto the title and make it colorful.
Most theme’s (not Connections templates) provide a method of adding custom CSS. Generally this is found within the theme Customizer. You can add any custom CSS you may want to add to that space.
RE: How to I structure the listings? I would like the names of the people to show on top. Then the name of the business (organization).
Sorry, I am not exactly sure what you are asking? When adding displaying an Organization entry, you want to display the Contact Name above the Organization name? Is that correct? If it is, the only way to change that would be to edit the PHP of the template.
Perhaps, add the entry as an Individual entry type and then add the business name as the Organization name instead. This will display the entry name above the organization name.
Hope this helps, let me know.