I use LESS quite a bit and most of our new sites are responsive in some manner.
What I love about LESS is a I can break down my CSS into individual files and then import/combine them and produce the final CSS file. Now I don't have to deal with a 2000+ line CSS file every time I want to make a small change. Going back and updating old projects that only use CSS and don't use LESS is so painful. Even just the ability to do single line comments is a godsend. Seriously, of all the languages that should have single line comments, CSS should be the one. But it doesn't. So frustrating.
Anyway, for example I'll always have a navigation.less file that contains only the styling for the navigation. This file also contains any media queries related to the menu.
I use a master.less file that imports all my other files and then just link to my master.css file in my HTML. Here's an example master.less file that I have in projects:
//Sizes
@container-width: 1250px;
@header-height: 137px;
@footer-height: 398px;
//Mobile Sizes
@desktop: 1250px;
@tablet-landscape-max: (@desktop - 1px); // 1249
@tablet-landscape-min: (@tablet-landscape-max - 225px); // 1024
@tablet-portrait-max: (@tablet-landscape-min - 1px); //1023
@tablet-portrait-min: (@tablet-portrait-max - 223px); //800
@mobile-large-max: (@tablet-portrait-min - 1px); //799
@mobile-large-min: (@mobile-large-max - 159px); //640
@mobile-small-max: (@mobile-large-min - 1px); // 639
@mobile-small-min: (@mobile-small-max - 159px); //480
@mobile-tiny: (@mobile-small-min - 1px); //479 or smaller
//Colours
@light-grey: #B4B4B4;
@light-grey2: #bdbebf;
@light-grey3: #D7D7D7;
@grey: #5a5a5a;
@dark-grey: #4A4A4A;
@green: #61bc46;
@green2: #3eb51b;
@green3: #40a123;
@orange: #fdbf3b;
@red: #FF0000;
@yellow: #FFDE16;
@error-background: #F9E0E0;
@error-border: #D60000;
@success-background: #D9EFD4;
@success-border: #1D7509;
@white: #FFFFFF;
@black: #000000;
//Fonts
@content-font: 'Lato', sans-serif;
@heading-font: 'Roboto Slab', serif;
//Miscellaneous
//Bring it all together
@import 'reset.less';
@import 'mixins.less';
@import 'global.less';
@import 'header.less';
@import 'footer.less';
@import 'sticky-footer.less';
@import 'navigation.less';
@import 'image-rotator.less';
@import 'home.less';
@import 'content.less';
@import 'posts.less';
@import 'galleries.less';
@import 'forms.less';
@import 'events.less';
@import 'reviews.less';
@import 'calendar.less';
We have used Bootstrap in the past but found it to be too restrictive so we just do our own responsive queries.