The Florence Welch-fronted band knocked Maroon 5 off the top spot to best their previous highest-charting entry, 2009's 'You've Got The Love', which reached number five.
Both debut album Lungs and 2011's follow-up Ceremonials, however, reached number one after their respective releases.
Maroon 5's 'Payphone' has been pushed down to two as a result, with will.i.am's 'This is Love' standing firm at three. 'Don't Wake Me Up' by Chris Brown drops two places to number four, while girl group Stooshe remain at five with 'Black Heart'.
Only two more new entries make the Top 40 today, as former American Idol star Adam Lambert sees his latest single 'Never Close Our Eyes' go straight in at 17. London indie rockers The Vaccines also squeeze into the chart at 37 with 'No Hope'.
The highest climbers this week are Rizzle Kicks, whose single 'Mama Do The Hump', originally released in December 2011, rockets up the chart to re-enter the Top 40 at 33. David Guetta's 'I Can Only Imagine', featuring Lil Wayne and Chris Brown, also shoots from 43 to 21.
Other tracks making their way back up the tally are LMFAO's 'Sexy and I Know It', up 17 places from 48 to 31, while Nicki Minaj's 'Pound the Alarm' achieves its highest chart placing to date, climbing from 16 to number ten.
Watch the video for 'Spectrum (Say My Name)' by Florence + the Machine below:
Source: Official Charts Company
> This week's albums chart